Terephthalate-intercalated nickel-aluminum layered double hydroxides (LDHs) were prepared by a co-precipitation method, with nominal x values in the general formula Ni((1-x))Al(x)(OH)(2)(C(8)H(4)O(4))(x/2) in the range 0.3-0.8. The materials were characterized by X-ray diffraction, X-ray fluorescence spectroscopy, CHN analysis, thermogravimetric analysis, FTIR spectroscopy, EXAFS at the Ni edge and (27)Al NMR spectroscopy. A combination of XRD, XRF and CHN analysis indicated that crystalline LDHs with true x values up to 0.5 were obtained, along with increasing segregation of an aluminum hydroxide phase with increasing aluminum content. The EXAFS analysis indicated an upper limit of ca. 0.6 for the atomic fraction of aluminum at the second nickel coordination sphere. The (27)Al NMR analysis suggested that a phase containing octahedrally co-ordinated Al(3+) is segregated for nominal x values from 0.6 upwards.